4.8 Article

Exciton-driven antiferromagnetic metal in a correlated van der Waals insulator

Journal

NATURE COMMUNICATIONS
Volume 12, Issue 1, Pages -

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41467-021-25164-8

Keywords

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Funding

  1. US Department of Energy, BES DMSE
  2. Gordon and Betty Moore Foundation's EPiQS Initiative [GBMF9459]
  3. National Science Foundation Graduate Research Fellowship [1745302]
  4. Swiss National Science Foundation [P2ELP2-172290, P400P2-183842]
  5. US Department of Energy [DE-SC0008739]
  6. Simons Investigator award from the Simons Foundation
  7. Pappalardo Fellowship at MIT
  8. Croucher Foundation Fellowship
  9. Institute for Basic Science (IBS) in Korea [IBS-R009-G1]
  10. Leading Researcher Program of the National Research Foundation of Korea [2020R1A3B2079375]
  11. National Research Foundation of Korea (NRF) - Ministry of Science, ICT, and Future Planning (MSIP) of Korea [NRF-2019R1I1A2A01062306, NRF-2017R1A5A1014862]
  12. Swiss National Science Foundation (SNF) [P400P2_183842, P2ELP2_172290] Funding Source: Swiss National Science Foundation (SNF)
  13. National Research Foundation of Korea [CG068702] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The authors demonstrate the generation of a transient metallic antiferromagnetic state in NiPS3 by non-equilibrium driving of spin-orbit-entangled excitons. This result highlights the unique properties of excitons in correlated insulators and suggests a potential avenue for optically manipulating magnetism through exciton-mediated processes.
Previous work has shown the existence of spin-orbit-entangled excitons and their coupling to antiferromagnetism in the correlated insulator NiPS3. Here the authors show that non-equilibrium driving of these excitons produces a transient metallic antiferromagnetic state that cannot be achieved by tuning the temperature in equilibrium. Collective excitations of bound electron-hole pairs-known as excitons-are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS3 by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and a long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism.

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